We have developed a gel-type surface-enhanced Raman scattering (SERS) sensor for the direct extraction of biomarkers from human skin and other sources. First, We used SERS-active sculptured Au nanoparticle substrates to explore how molecules move within hydroxyethyl cellulose (HEC) gels. This investigation aimed to understand the transport of biomarkers in gels and the feasibility of detecting them using SERS. Notably, the results revealed that HEC gels do not hinder SERS sensing. Additionally, the diffusion coefficient within the gels was found to be dependent on the molecular weight of the biomarkers. Then, we fabricated SERS-active sculptured thin-film dispersion gels by creating multilayer structures on mica. These multilayer structures significantly improved SERS performance due to the light confinement effect. Subsequently, we dispersed milled flakes into the gel. The resulting SERS-active flake dispersion gel holds promise for biosensing applications. Specifically, it allows for the direct collection of body fluids, such as sweat, from human skin.
In this study, we experimentally demonstrate the self-assembly of gold micropetals and microfluidic control thereof using their thermoplasmonic properties. To this end, gold micropetals were fabricated on a glass substrate via glancing angle deposition and microsphere lithography techniques. Each micropetal consisted of two portions with thin gold films of different thicknesses, resulting in an intrinsic optical absorption distribution. A water vapor microbubble was generated at the region of high optical absorption of the gold micropetal immersed in degassed water via irradiation from a CW laser. Subsequently, the thickness distribution on the micropetal yielded an effective temperature gradient along the substrate surface. Resultantly, the primary water stream around the bubble was tilted by ~45° from the surface normal. The micropetal is thus shown to be useful for providing a specific temperature gradient around the microbubble and generating a flow in the desired direction under the conditions of simple laser irradiation.
We experimentally investigated simultaneous microfluidic control and visualization of a heated region using gold nanoisland/VO2 thin films. By focusing a laser on the film, we photothermally generated an air microbubble in nondegassed water. After the bubble generation, another laser spot was irradiated 48 μm away from the bubble center. As a result, a sudden onset of the rotational Marangoni flow was observed at 130 ms after the laser was turned on. At the same time, the heated region above 70°C was visualized based on the thermochromic property of the thin film. The heated area did not vary significantly at the onset of the flow, indicating that there is a threshold temperature or temperature gradient on the bubble surface for generating the rotational Marangoni flow. To understand the flow generation, we decreased the distance between the bubble and the laser spot. The resulting visualized heated region suggests that a part of the bubble surface has to be heated above 70°C to generate the rotational flow. In addition, the heated area during the flow generation remained small as the distance decreased. The gold nanoisland/VO2 thin film is suitable for understanding and optimizing the rapid Marangoni flow generation.
We experimentally investigate the simultaneous microfluidic control and visualization of a heated region using gold nanoisland/VO2 thin films. Gold nanoisland/VO2 thin films are self-assembled using sputtering and glancing angle deposition techniques. The film shows a metal-insulator transition at approximately 70 °C. Therefore, the film is beneficial for visualizing the heated region inside the microfluidic chamber under a simple optical microscope. Furthermore, the photothermal property of the thin film enables a microbubble and a rapid Marangoni flow to be generated in water. The region heated above 70 °C around the bubble is visualized by the metal- insulator transition of the film. The visualization shows that the Marangoni flow is generated when a portion of the bubble is heated above 70 °C.
We experimentally investigated the manipulation of mica flakes using photothermally induced microbubbles. Iron silicide was sputtered on mica flakes to absorb the laser light and convert it to heat. By focusing a laser on to the flake immersed in degassed water, a water vapor microbubble was generated on the flake. The bubble involved strong Marangoni flow due to the steep temperature gradient on it. Laser irradiation at multiple spots allowed us to control the direction of the temperature gradient and subsequent Marangoni flow. By generating the flow parallel to the flake surface, the flake was driven on the glass substrate. This method is expected as a novel method to manipulate large and heavy particles in microfluidic channels.
We experimentally investigated the oscillation of the water vapor microbubble generated in degassed water using thermoplasmonic effect. A CW laser was focused on a gold nanoisland film to realize localized thermoplasmonic heating of the degassed water and subsequent generation of a water vapor microbubble. The generated bubble was found to be oscillating at 0.5{1 MHz although the laser power was constant. When the laser spot size, namely, the heating spot size, was fixed to 2.7 μm, the bubble diameter and the oscillation frequency was almost independent on the laser power. On the other hand, the bubble size significantly increased as the laser spot size increases from 2.8 to 3.7 μm. Besides, the oscillation frequency decreased as the bubble size increased, which was the same order of magnitude as the bubble resonance frequency. These results suggest that the behavior of the water vapor microbubble is highly dependent on the outmost region of the laser spot, to which the bubble contacts periodically.
The plasmonic nanostructures required for the SERS are commonly in the form of solid substrates, or as colloidal solutions, both of them are not very useful to detect the biomarkers directly on human skins. Gel-based SERS substrates, into which the plasmonic nanostructures are incorporated, will be helpful for the direct collection of the biomarkers from secretions such as sweat. To elucidate these points, we studied the diffusion of Raman probe 4, 4’-Bipyridine (BPY) in the cetyltrimethylammonium bromide:sodium salicylate (CTAB:NaSal) gel. Au nano-island SERS chip was coated with a 1:1 complex of CTAB:NaSal . Then, the diffusion of the probe was studied by SERS spectra as a function of time. The SERS signal intensity increases gradually with increasing time. Highly porous gel rapidly absorbed aqueous analyte solutions generating large SERS signals. The subsequent increase in signal could arise from the diffusion of the analyte molecule into the gel and onto the Au aggregates. Importantly, this gel-based SERS sensor did not significantly compromise the SERS performance of the analyte. We propose that this gel-based SERS sensor can be smeared directly onto the skin surface to absorb the body fluids from sweat, enabling the detection of biomarkers.
Access to the requested content is limited to institutions that have purchased or subscribe to SPIE eBooks.
You are receiving this notice because your organization may not have SPIE eBooks access.*
*Shibboleth/Open Athens users─please
sign in
to access your institution's subscriptions.
To obtain this item, you may purchase the complete book in print or electronic format on
SPIE.org.
INSTITUTIONAL Select your institution to access the SPIE Digital Library.
PERSONAL Sign in with your SPIE account to access your personal subscriptions or to use specific features such as save to my library, sign up for alerts, save searches, etc.